通过单个原子离子介导的甲和二氧化碳的同时功能化
Gaoxiang Liu1, Isuru R Ariyarathna2, Sandra M Ciborowski1
1Department of Chemistry, Johns Hopkins University, 3400 N Charles St, Baltimore, Maryland 21218,United States.
Journal of the American Chemical Society
|December 14, 2020
概括
这项研究显示单个离子同时激活甲和二氧化碳. 它通过将二氧化碳插入Pt-H和Pt-C键,形成新的分子,这是一个新的化学转化.
科学领域:
- 无机化学
- 催化剂
- 量子化学
背景情况:
- 甲和二氧化碳是重要的C1原料.
- 甲和二氧化碳的同时功能化仍然是催化的一个重大挑战.
- 离子金属复合物提供独特的反应途径.
研究的目的:
- 研究阴性 (Pt-),甲 (CH4) 和二氧化碳 (CO2) 的反应.
- 阐明单个原子离子同时激活CH4和CO2的机制.
- 为了确定由Pt,CH4和CO2相互作用而形成的产物.
主要方法:
- 对阳离子产物的质谱分析.
- 阳离子光电子光谱学
- 进行量子化学计算.
主要成果:
- 确定了甲激活复合物H3C-Pt-H.
- 这种复合物与二氧化碳发生反应,形成[H3C-Pt-H(CO2) ]-.
- 确定了两个化产物和一个C-C键合产物,它们都是[H3C-Pt-H[CO2]的异构体.
- 该机制涉及原子激活CH4和CO2.
- CO2 插入 Pt-H 和 Pt-C 键是由 Pt 上的电荷耗尽驱动的.
结论:
- 这项工作展示了由单个原子离子介导的同时CH4和CO2功能化的第一个例子.
- 这些发现突显了离子金属复合体在激活和转化稳定的小分子方面的潜力.
- 这项研究提供了由充电耗尽驱动的二氧化碳插入反应的机制见解.
更多相关视频
相关概念视频
Catalysis
29.2K
The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.
29.2K
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.7K
Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
3.7K
Reduction of Alkenes: Catalytic Hydrogenation
13.5K
Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
13.5K
Reduction of Alkynes to cis-Alkenes: Catalytic Hydrogenation
8.6K
Introduction
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
8.6K
Regioselectivity and Stereochemistry of Acid-Catalyzed Hydration
9.2K
The rate of acid-catalyzed hydration of alkenes depends on the alkene's structure, as the presence of alkyl substituents at the double bond can significantly influence the rate.
9.2K


